Sharing electronic and ionic transfer channels for high-energy-density and stable quasi-solid-state lithium-oxygen battery

Abstract Thick cathodes are essential for practical high-energy batteries, yet their development is hindered by sluggish charge kinetics, particularly in lithium-oxygen batteries (LOBs) where robust three-phase boundaries (TPBs) for e−, Li+, and O2 are indispensable. Herein, we propose a gel polymer electrolyte (GPE) integration strategy that enables the construction of a streamlined dual-conductive network for both e− and Li+ while preserving optimal porosity for rapid O2 diffusion in thick cathodes (~2 mm). This innovative architecture creates extensive and continuous TPBs throughout the entire cathode, enabling an exceptional areal capacity of 34.6 mAh cm−2, surpassing most previously reported LOBs, and a record-breaking gravimetric capacity of 19000 mAh g−1. Numerical simulations further validate the superiority of this approach. Our work provides a proof of concept for overcoming kinetic transport limitations in thick cathodes, paving the way for next-generation high-capacity and stable LOBs.